Non-oxidative activation of methane under a pulsed mode in the presence of supported platinum-containing catalysts

V. Pashkov, D. Golinsky, N. Vinichenko, A. Belyi
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Abstract

The novelty of the research was that the transformations were carried out in a pulsed mode at small contact times. A rise in temperature increases the amount of activated methane but decreases the H/C ratio in the surface hydrocarbon fragments. The optimal contact time of methane with the catalyst is in the range from 1 to 2.5 s. It provides the required methane activation depth and, which is most important, the optimal H/C ratio in the surface hydrocarbon fragments CHx equal to 3 at./at. An increase in the amount of strong LAS (a.b. at 2200 cm−1 and higher) in the support enhances methane activation at a considerable decrease in the H/C ratio in the surface hydrocarbon fragments, whereas a substantial increase (in the case of Pt/Al2O3−F, up to 150 μmol/g) deteriorates the activity toward methane activation and the H/C ratio.The novelty of the research was that the transformations were carried out in a pulsed mode at small contact times. A rise in temperature increases the amount of activated methane but decreases the H/C ratio in the surface hydrocarbon fragments. The optimal contact time of methane with the catalyst is in the range from 1 to 2.5 s. It provides the required methane activation depth and, which is most important, the optimal H/C ratio in the surface hydrocarbon fragments CHx equal to 3 at./at. An increase in the amount of strong LAS (a.b. at 2200 cm−1 and higher) in the support enhances methane activation at a considerable decrease in the H/C ratio in the surface hydrocarbon fragments, whereas a substantial increase (in the case of Pt/Al2O3−F, up to 150 μmol/g) deteriorates the activity toward methane activation and the H/C ratio.
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在负载型含铂催化剂的存在下,脉冲模式下甲烷的非氧化活化
该研究的新颖之处在于,转换是在脉冲模式下进行的,接触时间很短。温度升高会增加活性甲烷的数量,但会降低表面烃碎片的H/C比。甲烷与催化剂的最佳接触时间为1 ~ 2.5 s。它提供了所需的甲烷活化深度,最重要的是,表面烃碎片CHx的最佳H/C比等于3 at./at。在2200 cm−1及以上时,载体中强LAS (a.b.)含量的增加促进了甲烷的活化,而表面烃碎片的H/C比显著降低,而Pt/Al2O3−F含量的增加(高达150 μmol/g)则使甲烷活化活性和H/C比恶化。该研究的新颖之处在于,转换是在脉冲模式下进行的,接触时间很短。温度升高会增加活性甲烷的数量,但会降低表面烃碎片的H/C比。甲烷与催化剂的最佳接触时间为1 ~ 2.5 s。它提供了所需的甲烷活化深度,最重要的是,表面烃碎片CHx的最佳H/C比等于3 at./at。在2200 cm−1及以上时,载体中强LAS (a.b.)含量的增加促进了甲烷的活化,而表面烃碎片的H/C比显著降低,而Pt/Al2O3−F含量的增加(高达150 μmol/g)则使甲烷活化活性和H/C比恶化。
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